ChemCatChem
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2022
·Vol. 14
·期 12
·e202200274
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IF 5.497
Na Ji,Shuai Cheng,Zhichao Jia,Hanyang Li,Poknam Ri,Shurong Wang,Xinyong Diao
Graphical Working together : The establishment of Co 0 -Al 2 O 3 @USY interface via in-situ growth of CoAl-LDH on USY surface rendered the high activity in HDO of lignin to naphthenes which were attributed to the synergetic effect between Co 0 sites and USY, in which Co 0 sites were responsible for hydrogenation and acid sites on USY were responsible for deoxygenation. To enhance the catalytic activity and stability of metal catalysts in the hydrodeoxygenation of lignin derivatives into naphthenes, a bifunctional Co−Al 2 O 3 @USY catalyst was fabricated by the reduction of CoAl layered double hydroxide in-situ grown on the USY zeolite. In the hydrodeoxygenation of guaiacol, a 100.0 % conversion with cyclohexane yield up to 93.6 % was achieved at 180 °C, 3 MPa for 4 h, which should be the hitherto lowest reaction temperature that has been reported over Co-based metal catalysts. This catalyst was also relatively stable with 5 runs and exhibited excellent catalytic performance in the hydrodeoxygenation of other lignin model compounds and even real lignin feedstock into naphthenes. The high-efficiency of Co−Al 2 O 3 @USY was attributed to the synergistic effect between well-dispersed small Co nanoparticles and abundant acidic sites on the USY surface, while the outstanding stability was attributed to the anchoring effect of Al 2 O 3 matrix to Co nanoparticles which avoided the leaching of Co species and particle agglomeration. This work provides a potential strategy for the design of an efficient and stable catalyst for lignin utilization.
研究领域:
催化化学
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能源化学
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材料科学
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DOI
高影响因子
FUEL
·
2022
·
IF 8.035
Min Zhong,Pengju Yang,Bo Hou,Ming Xia,Jungang Wang
The main requirement for Co-based catalysts in Fischer-Tropsch synthesis (FTS) is to efficiently convert syngas (H 2 +CO) into long-chain hydrocarbons (C 5+ ). Since the formation of long-chain hydrocarbons (C 5+ ) is thermodynamically favored at low temperatures, it is desirable to develop efficient catalytic systems that can allow working at a relatively low reaction temperature. Herein, the Al 2 O 3 /Al composite has been used as support for the Co-based catalysts. The catalytic performance of Co/Al 2 O 3 /Al catalysts in FTS can be regulated by varying the Al 2 O 3 -layer thickness. With the thickening of Al 2 O 3 -layer, the catalytic activity and selectivity toward C 5+ hydrocarbons over Co/Al 2 O 3 /Al decrease markedly, although the number of accessible Co 0 sites increases obviously. This Al 2 O 3 -thickness-dependent FTS performance can be attributed to a variation of the proportion of active species Co-AlO x -Al and less active species Co-Al 2 O 3 . On the basis of the above finding, a highly active catalyst (Co/Al-0) has been developed using commercial Al metal powers as support, which will enable the FTS process to work at a fairly low reaction temperature (below 185 °C) and maintain excellent catalytic activity. This study provides a practical but low-cost method to modulate the electronic properties of metal catalysts by using available metal powders.
研究领域:
化学工程
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催化科学
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产品关联
DOI
高影响因子
Journal of CO2 Utilization
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2020
·
IF 5.993
Chengyi Dai,Xiao Zhao,Borui Hu,Xinbao Zhang,Qunxing Luo,Xinwen Guo,Xiaoxun Ma
Capturing and utilization of carbon dioxide (CO 2 ) not only leads to effective use of carbon resources, but also alleviates environmental pollution caused by increasing concentration of CO 2 , thus making it a hot research topic in recent years. In this study, a series of highly dispersed iron-cobalt (Fe-Co) catalysts was prepared by ethylenediaminetetraacetic acid disodium salt (EDTA-2Na) modification, which could efficiently convert CO 2 into high value-added chemicals (C 2 -C 4 = and C 5 -C 11 ). X-ray diffraction (XRD) analysis showed that the addition of a small amount of Co and EDTA-2Na contributed to enhance the sintering resistance of Fe species. During the calcination process, EDTA 4− can be decomposed into small organic molecules with reducibility, thus promoting the reduction of iron species. The CO temperature-programmed desorption (CO-TPD) results showed that cobalt enhanced the adsorption and activation of intermediate CO on Na x Fe-Co catalyst, thereby promoting the catalytic conversion of CO 2 . The complexation of EDTA promotes the synergistic effect of Fe-Co bimetals, enhances the chemical adsorption of CO 2 . Sodium in EDTA-2Na promotes the surface basicity of the catalysts, which is favored for improving the product distribution of hydrocarbons. At lower H 2 /CO 2 (1/1) ratio, the EDTA-2Na modified Fe-Co/Al 2 O 3 catalyst exhibited high conversion of CO 2 (32.8 %) and excellent selectivity toward high value-added chemicals. The selectivity of by-product CO was only 8.1 %; and C 2 -C 4 = (32.5 %) and C 5 -C 11 (46.3 %) accounted for ∼79 % selectivity among the hydrocarbons generated.
研究领域:
催化化学
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环境科学
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材料科学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Qunwei Guo,Xiaokun He,Jiaqi Geng,Jiawen Pan,Yuan Xue,Nan Xu,Bo Chi,Jian Pu
In this work, Ru is incorporated into Ni/Co to synthesize novel Al 2 O 3 -supported Ni-Ru/Co-Ru bimetallic catalysts. Tests verify their enhanced catalytic capability and durability and also reveal how each catalyst is deactivated. SEM and EDS results indicate that nanoparticle agglomeration on Ni-based surface triggers deactivation, and TG and XPS results suggest carbon deposition is fatal to Co-based catalysts. Implementing Ru effectively enhances catalytic activity and durability. To gain insight into the promoting effect of Ru, quantum mechanical methods are utilized to investigate the shifts in activation energies (E a ) in CH x * dehydrogenation processes on (1 1 1) surfaces. For the Ni catalyst, DFT calculations indicate that adding Ru decreases E a yet does not change the determining step. In contrast, adding Ru on the Co surface changes the major intermediates from CH* to CH 2 *, which inhibits further dehydrogenation , and hence mitigates carbon deposition to preserve the catalytic activity of the surface.
研究领域:
催化化学
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材料科学
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化学工程
·
量子化学
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能量转换
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DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2026
·
IF 3.9
Qi Zeng,Xinyi Xie,Cuilian Zhu,Lili Hu,Bo Xiao,Shupeng Guo,Bo Hou,Lili Liu,Min Zhong
The SiC NP-modified high thermal conductivity Co/Al2O3@Al Fischer–Tropsch synthesis (FTS) catalyst has been proven to significantly enhance catalytic activity and selectivity toward long-chain hydrocarbons (C5+), but the underlying mechanism responsible for this promotional effect remains unclear. In this study, commercially available SiO2 NPs are used as a substitute for SiC NPs to prepare a cost-effective SiO2-modified Co/Al2O3@Al catalyst (Co/AS-O) for improved FTS performance, serving as a reference to elucidate the unique role of SiC NPs in enhancing FTS performance. Systematic characterizations demonstrate that SiC promotes the formation of the hexagonal close-packed (HCP) Co phase, yielding a higher intrinsic activity. In contrast, the face-centered cubic (FCC) Co phase predominates in the Co/AS-O and an unmodified reference catalyst (Co/A-Y). Although both modified catalysts exhibit enhanced CO conversion, the superior activity of the SiC NP-modified catalyst (Co/AS-C) stems from an increased density of active sites and its higher intrinsic activity, as evidenced by a higher turnover frequency (TOF). In contrast, the enhancement for Co/AS-O is solely due to a greater number of exposed Co0 sites. Moreover, the incorporation of NPs enhances *CO adsorption and restricts the activity of surface *H species, collectively establishing a *C-rich microenvironment that promotes chain growth and olefin formation. This study provides a fundamental understanding of how inert NPs modulate the FTS performance of the thermally conductive Co/Al2O3@Al catalyst.
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DOI
高影响因子
ENERGY & FUELS
·
2026
·
IF 6
Jiuhong Wei,Yanni Liu,Shihua Zheng,Yajing Cai,Guojie Zhang
Dry reforming of methane (DRM) provides an attractive pathway for the simultaneous utilization of CH4 and CO2 to produce syngas; however, Co-based catalysts typically suffer from metal sintering, formation of hardly reducible cobalt aluminate (CoAl2O4), and severe carbon deposition under high-temperature conditions. Herein, Y-promoted Co catalysts supported on alumina with tailored pore architectures were developed, with particular emphasis on a hierarchical bimodal porous Al2O3 support (Al2O3-BA) integrating ordered mesopores and interconnected macroporous channels. Compared with mesoporous Al2O3-SA and commercial γ-Al2O3-supported counterparts, the 10Co-5Y/A2O3-BA catalyst exhibited smaller Co3O4 crystallites and more uniform nanoparticle dispersion, indicating mitigated agglomeration. H2-TPR analysis revealed enhanced reducibility with a shift of the main reduction peak to lower temperature and a markedly suppressed high-temperature CoAl2O4 feature, suggesting weakened metal–support interaction. CO2-TPD demonstrated an increased population of medium-strength basic sites, favoring CO2 adsorption and activation. XPS indicated a higher Co2+/Co3+ ratio and an increased proportion of surface-adsorbed oxygen species, implying modified surface electronic properties. These structural and surface characteristics translated into superior catalytic performance. The bimodal catalyst delivered the highest CH4 and CO2 conversions over 650–800 °C and maintained stable activity during a 24 h test at 750 °C, achieving 86.5% CH4 conversion, 91.5% CO2 conversion, and an H2/CO ratio of 0.92. Postreaction analyses revealed significantly reduced carbon deposition compared with mesoporous counterparts. Overall, the synergy between Y promotion and hierarchical bimodal porosity effectively modulates metal–support interaction, enhances reducibility and CO2 activation, and suppresses coking, providing a rational strategy for designing durable Co-based catalysts for DRM.
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产品关联
DOI
高影响因子
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